Multiple-scattering effects on incoherent neutron scattering in glasses and viscous liquids

Incoherent neutron scattering experiments are simulated for simple dynamic models: a glass (with a smooth distribution of harmonic vibrations) and a viscous liquid (described by schematic mode-coupling equations). In most situations multiple scattering has little influence upon spectral distributions, but it completely distorts the wavenumber-dependent amplitudes. This explains an anomaly observed in recent experiments

Vibrational States of Glassy and Crystalline Orthotherphenyl

Low-frequency vibrations of glassy and crystalline orthoterphenyl are studied by means of neutron scattering. Phonon dispersions are measured along the main axes of a single crystal, and the corresponding longitudinal and transversal sound velocities are obtained. For glassy and polycrystalline samples, a density of vibrational states is determined and cross-checked against other dynamic observables. In the crystal, low-lying zone-boundary modes lead to an excess over the Debye density of states. In the glass, the boson peak is located at even lower frequencies. With increasing temperature, both glass and crystal show anharmonicity.Comment: 7 pages of LaTeX (svjour), 2 tables, 10 figures accepted in Eur. Phys. J.

The Dynamic Transition of Protein Hydration Water

Thin layers of water on biomolecular and other nanostructured surfaces can be supercooled to temperatures not accessible with bulk water. Chen et al. [PNAS 103, 9012 (2006)] suggested that anomalies near 220 K observed by quasi-elastic neutron scattering can be explained by a hidden critical point of bulk water. Based on more sensitive measurements of water on perdeuterated phycocyanin, using the new neutron backscattering spectrometer SPHERES, and an improved data analysis, we present results that show no sign of such a fragile-to-strong transition. The inflection of the elastic intensity at 220 K has a dynamic origin that is compatible with a calorimetric glass transition at 170 K. The temperature dependence of the relaxation times is highly sensitive to data evaluation; it can be brought into perfect agreement with the results of other techniques, without any anomaly.Comment: 4 pages, 3 figures. Phys. Rev. Lett. (in press

Atomic Transport in Dense, Multi-Component Metallic Liquids

Pd43Ni10Cu27P0 has been investigated in its equilibrium liquid state with incoherent, inelastic neutron scattering. As compared to simple liquids, liquid PdNiCuP is characterized by a dense packing with a packing fraction above 0.5. The intermediate scattering function exhibits a fast relaxation process that precedes structural relaxation. Structural relaxation obeys a time-temperature superposition that extends over a temperature range of 540K. The mode-coupling theory of the liquid to glass transition (MCT) gives a consistent description of the dynamics which governs the mass transport in liquid PdNiCuP alloys. MCT scaling laws extrapolate to a critical temperature Tc at about 20% below the liquidus temperature. Diffusivities derived from the mean relaxation times compare well with Co diffusivities from recent tracer diffusion measurements and diffsuivities calculated from viscosity via the Stokes-Einstein relation. In contrast to simple metallic liquids, the atomic transport in dense, liquid PdNiCuP is characterized by a drastical slowing down of dynamics on cooling, a q^{-2} dependence of the mean relaxation times at intermediate q and a vanishing isotope effect as a result of a highly collective transport mechanism. At temperatures as high as 2Tc diffusion in liquid PdNiCuP is as fast as in simple liquids at the melting point. However, the difference in the underlying atomic transport mechanism indicates that the diffusion mechanism in liquids is not controlled by the value of the diffusivity but rather by that of the packing fraction

Propylene Carbonate Reexamined: Mode-Coupling β\beta Scaling without Factorisation ?

The dynamic susceptibility of propylene carbonate in the moderately viscous regime above $T_{\rm c}$ is reinvestigated by incoherent neutron and depolarised light scattering, and compared to dielectric loss and solvation response. Depending on the strength of $\alpha$ relaxation, a more or less extended $\beta$ scaling regime is found. Mode-coupling fits yield consistently $\lambda=0.72$ and $T_{\rm c}=182$K, although different positions of the susceptibility minimum indicate that not all observables have reached the universal asymptotics

Harmonic behavior of metallic glasses up to the metastable melt

In two amorphous alloys ZrTiCuNiBe and ZrAlNiCu coherent neutron scattering has been measured over five decades in energy, including measurements in the metastable melt of a metallic alloy more than 80 K above Tg. In the vibrational spectra a pronounced "boson" peak is found: Even in crystallized samples the density of states exceeds the Debye ω2 model, and in the amorphous state low-frequency vibrations are further enhanced. The peak position shows no dispersion in q, while intensities are strongly correlated with the static structure factor. Over the full energy range the temperature dependence is strictly harmonic. From high-energy resolution measurements we establish lower bounds for the temperatures at which structural α and fast β relaxation become observable

Sol-Gel Prepared Nanoscopic Metal Fluorides - a New Class of Tunable Acid-Base Catalysts

In this article, the high potential of the fluorolytic sol-gel process to synthesise nanoscopic metal fluorides with different acid-base properties is shown. These nanoscopic materials exhibit high potential to be used as heterogeneous catalysts due to their high surface areas and their tunable surface properties. Thus, for each specific reaction the required surface properties of the catalysts can be ”adjusted” to achieve a high yield and selectivity of the desired product. As a consequence, a greener method of chemical production can be accomplished. Moreover the cheap and easy synthesis of the catalysts using basic chemicals makes them not only interesting for fundamental research but provides an easy transformation to industrial applications

Wavenumber dependence of structural alpha relaxation in a molecular liquid

Structural alpha relaxation in liquid orthoterphenyl is studied by means of coherent neutron time-of-flight and backscattering spectroscopy over a large temperature range. Not only amplitude and relaxation time but also the spectral line shape show a significant variation with wavenumber. As expected from mode coupling theory, these variations are correlated with the static structure factor. Even far above the melting point, alpha relaxation remains non-exponential.Comment: 6 pages of LaTeX, 4 figure

Fast relaxation in a fragile liquid under pressure

The incoherent dynamic structure factor of ortho-terphenyl has been measured by neutron time-of-flight and backscattering technique in the pressure range from 0.1 MPa to 240 MPa for temperatures between 301 K and 335 K. Tagged-particle correlations in the compressed liquid decay in two steps. The alpha-relaxation lineshape is independent of pressure, and the relaxation time proportional to viscosity. A kink in the amplitude f_Q(P) reveals the onset of beta relaxation. The beta-relaxation regime can be described by the mode-coupling scaling function; amplitudes and time scales allow a consistent determination of the critical pressure P_c(T). alpha and beta relaxation depend in the same way on the thermodynamic state; close to the mode-coupling cross-over, this dependence can be parametrised by an effective coupling Gamma ~ n*T**{-1/4}.Comment: 4 Pages of RevTeX, 4 figures (submitted to Physical Review Letters

Molecular mode-coupling theory applied to a liquid of diatomic molecules

We study the molecular mode coupling theory for a liquid of diatomic molecules. The equations for the critical tensorial nonergodicity parameters ${\bf F}_{ll'}^m(q)$ and the critical amplitudes of the $\beta$ - relaxation ${\bf H}_{ll'}^m(q)$ are solved up to a cut off $l_{co}$ = 2 without any further approximations. Here $l,m$ are indices of spherical harmonics. Contrary to previous studies, where additional approximations were applied, we find in agreement with simulations, that all molecular degrees of freedom vitrify at a single temperature $T_c$. The theoretical results for the non ergodicity parameters and the critical amplitudes are compared with those from simulations. The qualitative agreement is good for all molecular degrees of freedom. To study the influence of the cut off on the non ergodicity parameter, we also calculate the non ergodicity parameters for an upper cut off $l_{co}=4$. In addition we also propose a new method for the calculation of the critical nonergodicity parameterComment: 27 pages, 17 figure